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How Mn/Ni Ordering ...
How Mn/Ni Ordering Controls Electrochemical Performance in High-Voltage Spinel LiNi0.44Mn1.56O4 with Fixed Oxygen Content
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- Aktekin, Burak (author)
- Uppsala universitet,Strukturkemi
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- Massel, Felix (author)
- Uppsala universitet,Molekyl- och kondenserade materiens fysik
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- Ahmadi, Majid (author)
- Delft Univ Technol, Fac Appl Sci, Kavli Inst Nanosci, NL-2628 CJ Delft, Netherlands.
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- Valvo, Mario (author)
- Uppsala universitet,Strukturkemi
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- Hahlin, Maria (author)
- Uppsala universitet,Molekyl- och kondenserade materiens fysik,Strukturkemi
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- Zipprich, Wolfgang (author)
- Volkswagen AG, D-38436 Wolfsburg, Germany.
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- Marzano, Fernanda (author)
- Scania CV AB, SE-15187 Sodertalje, Sweden.
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- Duda, Laurent (author)
- Uppsala universitet,Molekyl- och kondenserade materiens fysik
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- Younesi, Reza (author)
- Uppsala universitet,Strukturkemi
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- Edström, Kristina, Professor, 1958- (author)
- Uppsala universitet,Strukturkemi
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- Brandell, Daniel, 1975- (author)
- Uppsala universitet,Strukturkemi
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(creator_code:org_t)
- 2020-05-13
- 2020
- English.
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In: ACS Applied Energy Materials. - : AMER CHEMICAL SOC. - 2574-0962. ; 3:6, s. 6001-6013
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Abstract
Subject headings
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- The crystal structure of LiNi0.5O4 (LNMO) can adopt either low-symmetry ordered (Fd (3) over barm) or high-symmetry disordered (P4(3)32) space group depending on the synthesis conditions. A majority of published studies agree on superior electrochemical performance of disordered LNMO, but the underlying reasons for improvement remain unclear due to the fact that different thermal history of the samples affects other material properties such as oxygen content and particle morphology. In this study, ordered and disordered samples were prepared with a new strategy that renders samples with identical properties apart from their cation ordering degree. This was achieved by heat treatment of powders under pure oxygen atmosphere at high temperature with a final annealing step at 710 degrees C for both samples, followed by slow or fast cooling. Electrochemical testing showed that cation disordering improves the stability of material in charged (delithiated) state and mitigates the impedance rise in LNMO parallel to LTO (Li4Ti5O12) and LNMO parallel to Li cells. Through X-ray photoelectron spectroscopy (XPS), thicker surface films were observed on the ordered material, indicating more electrolyte side reactions. The ordered samples also showed significant changes in the Ni 2p XPS spectra, while the generation of ligand (oxygen) holes was observed in the Ni-O environment for both samples using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Moreover, high-resolution transmission electron microscopy (HRTEM) images indicated that the ordered samples show a decrease in ordering near the particle surface after cycling and a tendency toward rock-salt-like phase transformations. These results show that the structural arrangement of Mn/Ni (alone) has an effect on the surface and "nearsurface" properties of LNMO, particularly in delithiated state, which is likely connected to the bulk electronic properties of this electrode material.
Subject headings
- NATURVETENSKAP -- Kemi -- Materialkemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Materials Chemistry (hsv//eng)
Keyword
- high-voltage spinel
- LNMO
- cation ordering
- oxygen deficiency
- rock-salt
- anionic redox
Publication and Content Type
- ref (subject category)
- art (subject category)
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- By the author/editor
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Aktekin, Burak
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Massel, Felix
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Ahmadi, Majid
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Valvo, Mario
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Hahlin, Maria
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Zipprich, Wolfga ...
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show more...
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Marzano, Fernand ...
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Duda, Laurent
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Younesi, Reza
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Edström, Kristin ...
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Brandell, Daniel ...
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- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Materials Chemis ...
- Articles in the publication
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ACS Applied Ener ...
- By the university
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Uppsala University